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High-Productivity Continuous Conversion of Glucose to α-Hydroxy Esters over Postsynthetic and Hydrothermal Sn-Beta Catalysts

[Image: see text] The retro-aldol fragmentation of glucose is a complex reaction of industrial relevance, which provides a potentially sustainable route for the production of α-hydroxyester compounds of relevance to the green polymer industry, such as methyl lactate and methyl vinyl glycolate. Altho...

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Autores principales: Botti, Luca, Navar, Ricardo, Tolborg, Søren, Martínez-Espín, Juan S., Hammond, Ceri
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2022
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9007564/
https://www.ncbi.nlm.nih.gov/pubmed/35433137
http://dx.doi.org/10.1021/acssuschemeng.1c06989
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author Botti, Luca
Navar, Ricardo
Tolborg, Søren
Martínez-Espín, Juan S.
Hammond, Ceri
author_facet Botti, Luca
Navar, Ricardo
Tolborg, Søren
Martínez-Espín, Juan S.
Hammond, Ceri
author_sort Botti, Luca
collection PubMed
description [Image: see text] The retro-aldol fragmentation of glucose is a complex reaction of industrial relevance, which provides a potentially sustainable route for the production of α-hydroxyester compounds of relevance to the green polymer industry, such as methyl lactate and methyl vinyl glycolate. Although the zeolite catalyst, Sn-Beta, has shown itself to be a promising catalyst for this process, important information concerning the stability of the catalyst during continuous operation is not yet known, and improvements to its yield of retro-aldol products are also essential. Here, we perform detailed spectroscopic studies of a selection of Sn-Beta catalysts and evaluate their performances for the retro-aldol fragmentation of glucose under continuous processing conditions, with the dual aims of developing new structure–activity–lifetime relationships for the reaction and maximizing the productivity and selectivity of the process. Kinetic studies are performed under both established reaction conditions and in the presence of additional promoters, including water and alkali salts. Generally, this study demonstrates that the reaction conditions and choice of catalyst cannot be optimized in isolation, since each catalyst explored in this study responds differently to each particular process perturbation. However, by evaluating each type of the Sn-Beta catalyst under each set of reaction conditions, we reveal that postsynthetic Sn-Beta catalysts exhibit the best levels of performance when activity, selectivity, and stability are taken into account. Specifically, the best levels of performance are obtained with a postsynthetic Sn-Beta catalyst that is preactivated in a flow of methanol prior to reaction, which provides α-hydroxyester yields over 90% at the early stages of continuous operation and operates at high yield and selectivity for over 60 h on stream. Space–time-yields over two orders of magnitude higher than any previously reported for this reaction are achieved, setting a new benchmark in terms of the retro-aldol fragmentation of glucose.
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spelling pubmed-90075642022-04-14 High-Productivity Continuous Conversion of Glucose to α-Hydroxy Esters over Postsynthetic and Hydrothermal Sn-Beta Catalysts Botti, Luca Navar, Ricardo Tolborg, Søren Martínez-Espín, Juan S. Hammond, Ceri ACS Sustain Chem Eng [Image: see text] The retro-aldol fragmentation of glucose is a complex reaction of industrial relevance, which provides a potentially sustainable route for the production of α-hydroxyester compounds of relevance to the green polymer industry, such as methyl lactate and methyl vinyl glycolate. Although the zeolite catalyst, Sn-Beta, has shown itself to be a promising catalyst for this process, important information concerning the stability of the catalyst during continuous operation is not yet known, and improvements to its yield of retro-aldol products are also essential. Here, we perform detailed spectroscopic studies of a selection of Sn-Beta catalysts and evaluate their performances for the retro-aldol fragmentation of glucose under continuous processing conditions, with the dual aims of developing new structure–activity–lifetime relationships for the reaction and maximizing the productivity and selectivity of the process. Kinetic studies are performed under both established reaction conditions and in the presence of additional promoters, including water and alkali salts. Generally, this study demonstrates that the reaction conditions and choice of catalyst cannot be optimized in isolation, since each catalyst explored in this study responds differently to each particular process perturbation. However, by evaluating each type of the Sn-Beta catalyst under each set of reaction conditions, we reveal that postsynthetic Sn-Beta catalysts exhibit the best levels of performance when activity, selectivity, and stability are taken into account. Specifically, the best levels of performance are obtained with a postsynthetic Sn-Beta catalyst that is preactivated in a flow of methanol prior to reaction, which provides α-hydroxyester yields over 90% at the early stages of continuous operation and operates at high yield and selectivity for over 60 h on stream. Space–time-yields over two orders of magnitude higher than any previously reported for this reaction are achieved, setting a new benchmark in terms of the retro-aldol fragmentation of glucose. American Chemical Society 2022-03-30 2022-04-11 /pmc/articles/PMC9007564/ /pubmed/35433137 http://dx.doi.org/10.1021/acssuschemeng.1c06989 Text en © 2022 American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Botti, Luca
Navar, Ricardo
Tolborg, Søren
Martínez-Espín, Juan S.
Hammond, Ceri
High-Productivity Continuous Conversion of Glucose to α-Hydroxy Esters over Postsynthetic and Hydrothermal Sn-Beta Catalysts
title High-Productivity Continuous Conversion of Glucose to α-Hydroxy Esters over Postsynthetic and Hydrothermal Sn-Beta Catalysts
title_full High-Productivity Continuous Conversion of Glucose to α-Hydroxy Esters over Postsynthetic and Hydrothermal Sn-Beta Catalysts
title_fullStr High-Productivity Continuous Conversion of Glucose to α-Hydroxy Esters over Postsynthetic and Hydrothermal Sn-Beta Catalysts
title_full_unstemmed High-Productivity Continuous Conversion of Glucose to α-Hydroxy Esters over Postsynthetic and Hydrothermal Sn-Beta Catalysts
title_short High-Productivity Continuous Conversion of Glucose to α-Hydroxy Esters over Postsynthetic and Hydrothermal Sn-Beta Catalysts
title_sort high-productivity continuous conversion of glucose to α-hydroxy esters over postsynthetic and hydrothermal sn-beta catalysts
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9007564/
https://www.ncbi.nlm.nih.gov/pubmed/35433137
http://dx.doi.org/10.1021/acssuschemeng.1c06989
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